Separation and Purification Technology ( IF 8.1 ) Pub Date : 2022-06-26 , DOI: 10.1016/j.seppur.2022.121564 Kaicheng Yang , Tianxia Liu , Dingzhou Xiang , Youji Li , Zhiliang Jin
Graphdiyne (GDY), as a novel two-dimension carbon allotrope material composed of sp- and sp2-hybrid carbon network, has been widely explored since it was synthesized for the first time by Li’s group in 2010. In this research, we developed a synthesis scheme of Co3S4-anchored graphdiyne/carbon defects g-C3N4 (DCN) nano-hybrids for efficient photocatalytic hydrogen evolution. This system has a fantastic 0D-2D/2D structure and the porous interconnected framework favors multivariate collaborative catalysis, greatly promoting the mass transfer performance between them, and enhancing the light absorption and the density of active sites. Most of all, as a charge transfer station, the edge-covalently modified GDY provides shortcuts for the dual-induction of electrons and holes. Charge kinetic analysis indicated that the electron transfer rate of the system reached 9.27 × 109 s−1, and the ultra-fast interfacial transfer considerably promoted the charge separation. In addition, photoelectrochemical technology verified that the multiplex nanoreactor has lower carrier recombination rate and smaller hydrogen evolution overpotential. Under 5 W LED light (λ > 420 nm), the dye-sensitized optimized hydrogen generation rate is 2075.67 μmol g−1 h−1, which is 77.2 times that of bare DCN. This work is expected to develop a new design concept for the construction of multiple and efficient synergistic nanocomposites, opening up new opportunities and possibilities for photocatalysis applications.
中文翻译:
基于石墨二炔 (g-CnH2n-2) 的 Co3S4 锚定和边缘共价修饰结合碳缺陷 g-C3N4 用于光催化制氢
石墨二炔(GDY)作为一种由sp-和sp 2 -杂化碳网络组成的新型二维碳同素异形体材料,自李氏课题组2010年首次合成以来,得到了广泛的探索。 Co 3 S 4锚定的石墨二炔/碳缺陷gC 3 N 4的合成方案(DCN) 纳米杂化物用于高效的光催化析氢。该体系具有奇妙的0D-2D/2D结构,多孔互连框架有利于多元协同催化,极大地促进了它们之间的传质性能,提高了光吸收和活性位点的密度。最重要的是,作为电荷转移站,边缘共价修饰的 GDY 为电子和空穴的双重感应提供了捷径。电荷动力学分析表明体系的电子转移速率达到9.27×10 9 s -1,超快的界面转移极大地促进了电荷分离。此外,光电化学技术验证了多重纳米反应器具有较低的载流子复合率和较小的析氢过电位。在5 W LED光(λ > 420 nm)下,染料敏化优化的产氢率为2075.67 μmol g -1 h -1,是裸DCN的77.2倍。这项工作有望为构建多种高效协同纳米复合材料开发一种新的设计理念,为光催化应用开辟新的机遇和可能性。